The hydrazine oxidation-assisted H evolution method promises low-input and input-free hydrogen production. However, developing high-performance catalysts for hydrazine oxidation (HzOR) and hydrogen evolution (HER) is challenging. Here, we introduce a bifunctional electrocatalyst α-MoC/N-C/Ru, merging ruthenium (Ru) nanoclusters (NCs) and single atoms (SA) into cubic α-MoC nanoparticles-decorated N-doped carbon (α-MoC/N-C) nanowires, through electrodeposition.
View Article and Find Full Text PDFWhile Ru owns superior catalytic activity toward hydrogen oxidation reaction and cost advantages, the catalyst deactivation under high anodic potential range severely limits its potential to replace the Pt benchmark catalyst. Unveiling the deactivation mechanism of Ru and correspondingly developing protection strategies remain a great challenge. Herein, we develop atomic Pt-functioned Ru nanoparticles with excellent anti-deactivation feature and meanwhile employ advanced operando characterization tools to probe the underlying roles of Pt in the anti-deactivation.
View Article and Find Full Text PDFChem Commun (Camb)
November 2023
The high unoccupied d band energy of FeS basically results in weak orbital coupling with water molecules, consequently leading to sluggish water dissociation kinetics. Herein, we demonstrate that the N-induced doping effect and phase transition engineering (FeS to N-FeS) can downshift the unoccupied d orbitals and strengthen the interfacial orbital coupling to boost the water dissociation kinetics. The fabricated N-FeS/carbon cloth (CC) displays superb hydrogen evolution reaction performance with a low overpotential (89 mV at 10 mA cm) and small Tafel slope (105 mV dec) under alkaline conditions.
View Article and Find Full Text PDFLuminescent metal clusters have attracted great interest in current research; however, the design synthesis of Al clusters with color-tunable luminescence remains challenging. Herein, an [Al (OH) (NA) ] (Al , HNA = nicotinic acid) molecular cluster with dual luminescence properties of fluorescence and room-temperature phosphorescence (RTP) is synthesized by choosing HNA ligand as phosphor. Its prompt photoluminescence (PL) spectrum exhibits approximately white light emission at room temperature.
View Article and Find Full Text PDFCation exchange (CE) in metal oxides under mild conditions remains an imperative yet challenging goal to tailor their composition and enable practical applications. Herein, we first develop an amorphization-induced strategy to achieve room-temperature CE for universally synthesizing single-atom doped InO nanosheets (NSs). Density functional theory (DFT) calculations elucidate that the abundant coordination-unsaturated sites present in a-InO NSs are instrumental in surmounting the energy barriers of CE reactions.
View Article and Find Full Text PDFWater electrolysis for H production is restricted by the sluggish oxygen evolution reaction (OER). Using the thermodynamically more favorable hydrazine oxidation reaction (HzOR) to replace OER has attracted ever-growing attention. Herein, we report a twisted NiCoP nanowire array immobilized with Ru single atoms (Ru -NiCoP) as superior bifunctional electrocatalyst toward both HzOR and hydrogen evolution reaction (HER), realizing an ultralow working potential of -60 mV and overpotential of 32 mV for a current density of 10 mA cm , respectively.
View Article and Find Full Text PDFTransition metal oxides with high theoretical capacities are promising anode materials for lithium-ion batteries (LIBs). However, the sluggish reaction kinetics remain a bottleneck for fast-charging applications due to its slow Li migration rate. Herein, a strategy is reported of significantly reducing the Li diffusion barrier of amorphous vanadium oxide by constructing a specific ratio of the VO local polyhedron configuration in amorphous nanosheets.
View Article and Find Full Text PDFThe use of polyoxometalate clusters (POMs) with multitudinous structures and surface properties as building blocks has sparked the development of cluster-assembled materials with many prospective applications. In comparison to classic molecules and assembly processes, control over the steric interactions and linkage of large POMs to achieve superlattices with multiple levels of organization remains a great challenge. This work presents a universal approach to modulate the spatial coordination behavior and configurations, and achieves a class of cluster superlattice architectures formed by linear alignment and two-dimensional arrangement of POM units.
View Article and Find Full Text PDFThe transformation of dietary structure brought about by economic development in populous countries is expected to trigger an increase in grain demand, which will put enormous pressure on the grain supply in these nations and even globally. We simulated nine demand scenarios for 2020-2050 based on China's dataset for 15 kinds of grains from 1961-2018. The results show that the maximum difference between the predicted grain demand is 323.
View Article and Find Full Text PDFPrecisely constructing the local configurations of active sites to achieve on-demand catalytic functions is highly critical yet challenging. Herein, an anion-deficient strategy to precisely capture Ru single atoms on the anion vacancies of CoP (Ru-SA/Pv-CoP ) is developed. Refined structural characterizations reveal that the Ru single atoms preferably bind to the anion vacancy sites and consequently build a superior catalytic surface with neighboring CoP and CoRu coordination states for the hydrogen evolution reaction (HER) catalysis.
View Article and Find Full Text PDFThe capability of manipulating the interfacial electronic coupling is the key to achieving on-demand functionalities of catalysts. Herein, it is demonstrated that the electronic coupling of Fe N can be effectively regulated for hydrogen evolution reaction (HER) catalysis by vacancy-mediated orbital steering. Ex situ refined structural analysis reveals that the electronic and coordination states of Fe N can be well manipulated by nitrogen vacancies, which impressively exhibit strong correlation with the catalytic activities.
View Article and Find Full Text PDFP-rich transition metal phosphides (TMPs) with abundant P sites have been predicted to be more favorable for hydrogen evolution reaction (HER) catalysis. However, the actual activities of P-rich TMPs do not behave as expected, and the underlying essence especially at the atomic level is also ambiguous. Our structural analysis reveals the inferior activity could stem from the reduced overlap of atomic wave functions between metal and P with the increase in P contents, which consequently results in too strong P-H interaction.
View Article and Find Full Text PDFMolybdenum disulfide is naturally inert for alkaline hydrogen evolution catalysis, due to its unfavorable water adsorption and dissociation feature originated from the unsuitable orbital orientation. Herein, we successfully endow molybdenum disulfide with exceptional alkaline hydrogen evolution capability by carbon-induced orbital modulation. The prepared carbon doped molybdenum disulfide displays an unprecedented overpotential of 45 mV at 10 mA cm, which is substantially lower than 228 mV of the molybdenum disulfide and also represents the best alkaline hydrogen evolution catalytic activity among the ever-reported molybdenum disulfide catalysts.
View Article and Find Full Text PDFAlthough it is commonly believed that the water-dissociation-related Volmer process is the rate-limiting step for alkaline hydrogen evolution reaction (HER) on Pt-based catalysts, the underlying essence, particularly on the atomic scale, still remains unclear. Herein, it is revealed that the sluggish water-dissociation behavior probably stems from unfavorable orbital orientation and the kinetic issue is successfully resolved via N-induced orbital tuning. Impressively, N modified Pt-Ni nanowires deliver an ultralow overpotential of 13 mV at 10 mA cm , which represents a new benchmark for alkaline HER catalysis.
View Article and Find Full Text PDFMetal sulfides for hydrogen evolution catalysis typically suffer from unfavorable hydrogen desorption properties due to the strong interaction between the adsorbed H and the intensely electronegative sulfur. Here, we demonstrate a general strategy to improve the hydrogen evolution catalysis of metal sulfides by modulating the surface electron densities. The N modulated NiCoS nanowire arrays exhibit an overpotential of 41 mV at 10 mA cm and a Tafel slope of 37 mV dec, which are very close to the performance of the benchmark Pt/C in alkaline condition.
View Article and Find Full Text PDFEndowing materials with specific functions that are not readily available is always of great importance, but extremely challenging. Co N, with its beneficial metallic characteristics, has been proved to be highly active for the oxidation of water, while it is notoriously poor for catalyzing the hydrogen evolution reaction (HER), because of its unfavorable d-band energy level. Herein, we successfully endow Co N with prominent HER catalytic capability by tailoring the positions of the d-band center through transition-metal doping.
View Article and Find Full Text PDFBased on 1128 survey questionnaires, main information on urban and rural household electricity consumption was obtained. Original data included household income, the price of electricity, all kinds of electrical appliances, purchase price of main appliances, household size, electricity consumption, as well as power, daily use time of electrical appliances in this data article. These data fully reflected behavior, preferences and living pattern of sample households in electricity use and provided the basis for analyzing the relationship between household electricity consumption and the quality of life ("Does electricity consumption improve residential living status in less developed regions? An empirical analysis using the quantile regression approach" [1]).
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